Browsing by Subject "Nanoplatelets"

Now showing 1 - 20 of 24

Open Access
CdSe/CdMnS nanoplatelets with bilayer core and magnetically doped shell exhibit switchable excitonic circular polarization: Implications for lasers and light-emitting diodes
(American Chemical Society, 2020-03) Najafi, A.; Tarasek, S.; Delikanlı, Savaş; Zhang, P.; Norden, T.; Shendre, S.; Sharma, Manoj; Bhattacharya, A.; Taghipour, Nima; Pientka, J.; Dedmir, Hilmi Volkan; Thomay, T.
We utilized time-resolved photoluminescence (TRPL) spectroscopy to study the excitonic circular polarization (PX) from CdSe/CdMnS core/shell nanoplatelets (NPLs) with a bilayer core. This allows an extensive study of the emission dynamics as a function of magnetic field, temperature, doping concentration, and excitation wavelength. In the presence of an external magnetic field, pulsed excitation below the shell gap results in near-zero excitonic circular polarization PX at all time delays. In contrast, pulsed excitation with photon energy larger than the shell gap results in a rapid (100 ps) buildup of the excitonic circular polarization which subsequently remains constant at a level of up to 40%. We propose a model to describe the dynamics which takes into account the exchange interaction between carrier and magnetic ion (Mn) spins. The studied system exhibits a fast switchable excitonic circular polarization, implying possible applications in lasers and light emitting diodes.
Open Access
Colloidal photonics of semiconductor nanocrystals: from polarized color conversion to efficient solar concentration
(2018-07) Güngör, Kıvanç
Effective photon management is pivotal to the success of future photonic applications. The demand for high-performance electronic displays and solar light harvesters has been increasingly growing, ever with high expectations in advancing their power efficiencies. Semiconductor nanocrystals are highly promising for use in such advanced photonic applications. However, conventional device architectures and fabrication methods cannot fully exploit their potential. To address the need for their effective utilization, in this thesis, we proposed and demonstrated novel photon managing methods for colloidal nanocrystals to target polarized color conversion and efficient solar concentration. Nanocrystals possess an unmatched color purity for next-generation displays but color enrichment in displays suffers from the inherent random polarization in their photoluminescence. Instead of clipping the undesired polarization, we show a new class of v-shaped backlight unit (v-BLU) creating Fano resonances to enforce isotropic quantum emitters of the integrated color-conversion nanocrystals to emit polarized light. While enabling a front-panel configuration, the proposed v-BLU of nanocrystals allows for a strong modification of the density of optical states via resonance coupling. This control over the density of states for isotropic quantum dots empowers the realization of high polarization contrast ratios while sustaining their optical transmission. Similar to color conversion, colloidal nanocrystals are also instrumental to light harvesting, in particular using atomically at nanocrystals with their step-like absorption profile making them potentially ideal candidates for luminescent solar concentrators (LSCs). Nevertheless, practically zero Stokes shift in their photoluminescence fundamentally limits their utilization. Here we overcame this limitation by proposing the doping of such colloidal quantum wells inducing a large Stokes shift with near-unity photoluminescence quantum efficiency. We developed and demonstrated high-performance LSC panels of the copper-doped quantum wells outperforming the LSCs of their undoped counterparts and doped quantum dots. The LSCs of such Cu-doped quantum wells offer record optical flux gain compared to other colloids. We believe that the findings presented in this thesis will advance the applications of colloidal nanocrystals boosting the performance of their next-generation photonic devices to unprecedented levels.
Open Access
Colloidal synthesis and doping of semiconductor nanocrystals
(2015-07) Akgül, Mehmet Zafer
Colloidal semiconductor nanocrystals have drawn great interest for application areas in photonics and optoelectronics thanks to their superior optical properties including strong bandgap emission and tunability. Also, their suitability for solution-based processing has made them highly attractive for low-cost production of light-emitting diodes and lasers. Our objective in this thesis is to show the potential and versatility of semiconductor nanocrystals via colloidal synthesis and post-processing methods. The thesis work includes the synthesis of colloidal quantum dot and well structures and their post-doping and investigates their exciton decay dynamics. In this thesis a novel colloidal approach for the doping of zinc blende colloidal quantum wells was proposed and demonstrated for the first time. This new doping method uniquely relies on atomic layer deposition (ALD) process. Here we achieved the worlds first manganese-doped CdSe@CdS core@shell nanoplatelets using our technique of ALD-assisted doping. Also, we studied silver-doped CdTe quantum dots under different conditions. Our experimental work proved that the quantum yield enhancement of silver-doped CdTe quantum dots is a strong function of the nanocrystal size and doping concentration. Tuning the nanocrystal size and doping level, our aqueous core-only CdTe nanocrystals reached a record high photoluminescence quantum efficiency of 68%. For these quantum dots, various decay kinetics were proposed and the enhancement in the quantum yield was attributed to the trap state annihilation. The methods and results provided in this thesis contribute to the fundamental understanding of semiconductornanocrystals and pave the way for high-performance colloidal platforms and devices.
Embargo
Colloidal synthesis and optical properties of heterostructured quantum wells
(2024-08) Işık, Furkan
Colloidal quantum wells (CQWs) have emerged as auspicious gain materials for next-generation colloidal nanolasers owing to their exceptional optoelectronic properties including intrinsically suppressed Auger recombination, large absorption cross-section, low cost of production, and the ability to precisely tailor their attributes. However, the realization of their photonic devices faces fundamental challenges inherent to semiconductor nanocrystals in general, which can be tackled via the design and engineering of their advanced heterostructures. In this thesis, we proposed multiple design strategies to address scientific obstacles associated with using such CQWs as gain materials and developed a variety of their rational heterostructure designs by implementing advanced synthesis techniques, allowing us to systematically study the structure-property relationship. We investigated the optical gain performance of these CQW heterostructures through spectral and temporal spectroscopy techniques to elucidate the underlying mechanisms, which guided us to improve the associated structural aspects of CQWs. This approach culminated in the development of superior CQW heterostructures possessing low optical gain thresholds, giant material gain coefficients, and long gain lifetimes, addressing all main specifications quantifying the quality of a gain material. We also presented proof-of-concept device demonstrations showcasing the advancement in the gain aspect of these CQW heterostructures, such as high-performance amplified spontaneous emission in solution and whispering gallery mode lasing with ultra-low thresholds. The findings of this thesis indicate highly engineered CQW heterostructures offer excellent gain media.
Open Access
Colloidal synthetic pathways of atomically-flat complex nanocrystal heterostructures
(2024-01) Shabani, Farzan
Colloidal semiconductor nanocrystals (NCs) constitute one of the most important branches of nanoscience, with an increasingly high research interest, culminating with a Nobel Prize most recently. The nanometric size of these NCs allows for size-dependent optical properties, which provides an extra tool besides the composition to fine-tune these properties. Recent advancements in NC synthesis have been enabling important developments in the design and engineering of different shapes, compositions, and heterostructures of NCs. Accompanied by a deeper physical understanding and more sophisticated fabrication techniques, the NCs are now being integrated into many of the optoelectronic devices and are of prime importance for the next-generation optoelectronics. Despite all the progress, however, the full potential and synthesis dynamics of the NCs still need further investigation. Here, we addressed specifically four key aspects of the semiconductor NCs: shape engineering, electronic heterostructures, doping, and surface modification. In this thesis research, the synthesis dynamics, especially nucleation, growth and diffusion, were investigated in depth for different synthetic routes and conditions, and some of the important challenges were resolved. With the scarce number of proper emitters at longer wavelengths, in this thesis, a complex and thick heterostructure based on group II-VI nanoplatelets (NPLs) with relaxed quantum confinement was developed. The multi-shell design of the proposed NPLs helps overcome the unfavorable growth in the thickness direction, which, together with the cation dissolution/recrystallization and cation reorganization at high temperatures, relaxes the strain between the domains. The final NPLs, emitting in the deep-red region close to the bulk bandgap of CdSe, were used as an active layer in a light-emitting diode (LED) device and exhibited an exceptionally high external quantum efficiency (EQE) of 6.8% at electroluminescence peak wavelength of 701 nm, one of the best reported for colloids in this spectral range in the literature. Additionally, a novel heterostructure of multi-crown NPLs was designed and demonstrated, where several direct and indirect recombination pathways give rise to photoluminescence with both type-I and type-II characteristics. The design of these NPLs, especially the size of the domains, was shown to significantly impact the final optical properties that can activate/deactivate the recombination channels alongside the temperature. These multi-crown type-II NPLs exhibit an extremely high two-photon absorption cross-section with the highest value of 12.9 × 106 GM and low dark-bright exciton splitting energy critical for optoelectronic applications, including photodetectors, bioimaging and quantum devices. Next, we showed silver doping dynamics of core/shell NPLs, which previously proved challenging due to the self-purification after the shell growth. Here, the composition of the shell was shown to be an important factor in the destruction mechanism of the NPLs in the irreversible doping regime at high doping temperatures. The Ag:CdSe/CdZnS core/shell NPLs exhibit only dopant emission with superior paramagnetic properties compared to CdS-shelled NPLs thanks to better lattice preservation and higher dopant content. At last, a surface modification method was suggested and demonstrated for group I-III-VI NCs to enhance their electronic properties. Replacing the long-chain organic ligands with a S2- layer, injection of a negative charge and passivation of donor sites changed the behavior of the field-effect transistors (FETs) based on these NCs from p-type to n-type with more than a 105-fold enhancement in the carrier mobility. This method allowed fine-tuning of the optical properties of the NCs by the diffusion of the cations and shell formation. The findings of this thesis shine light on some of the important challenges in the field of semiconductor NCs while drawing a guideline for future research on the synthetic routes and optoelectronic properties. The thesis paves the way for future device integration of the developed NCs to fully realize their potential, while the demonstration of the more elaborated properties, including nonlinear absorption, paramagnetism and dark-bright exciton splitting, encourages further fundamental studies focusing on the physics of the semiconductor NCs.
Open Access
Color enrichment solids of spectrally pure colloidal quantum wells for wide color Span in displays
(Wiley-VCH Verlag GmbH & Co. KGaA, 2022-07-18) Erdem, T.; Soran Erdem, Z.; Işık, Furkan; Shabani, Farzan; Yazici, A. F.; Mutlugün, E.; Gaponik, N.; Demir, H. V.
Colloidal quantum wells (CQWs) are excellent candidates for lighting and display applications owing to their narrow emission linewidths (<30 nm). However, realizing their efficient and stable light-emitting solids remains a challenge. To address this problem, stable, efficient solids of CQWs incorporated into crystal matrices are shown. Green-emitting CdSe/CdS core/crown and red-emitting CdSe/CdS core/shell CQWs wrapped into these crystal solids are employed as proof-of-concept demonstrations of light-emitting diode (LED) integration targeting a wide color span in display backlighting. The quantum yield of the green- and red-emitting CQW-containing solids of sucrose reach ≈20% and ≈55%, respectively, while emission linewidths and peak wavelengths remain almost unaltered. Furthermore, sucrose matrix preserves ≈70% and ≈45% of the initial emission intensity of the green- and red-emitting CQWs after >60 h, respectively, which is ≈4× and ≈2× better than the drop-casted CQW films and reference (KCl) host. Color-converting LEDs of these green- and red-emitting CQWs in sucrose possess luminous efficiencies 122 and 189 lm W−1elect, respectively. With the liquid crystal display filters, this becomes 39 and 86 lm W−1elect, respectively, providing with a color gamut 25% broader than the National Television Standards Committee standard. These results prove that CQW solids enable efficient and stable color converters for display and lighting applications.
Open Access
Coreless fiber‐based whispering‐gallery‐mode assisted lasing from colloidal quantum well solids
(Wiley-VCH Verlag, 2020-01) Sak, Mustafa; Taghipour, Nima; Delikanlı, Savaş; Shendre, S.; Tanrıöver, İbrahim; Gao, Y.; Yu, J.; Yanyan, Z.; Yoo, S.; Dang, C.; Demir, Hilmi Volkan; Foroutan, Sina
Whispering gallery mode (WGM) resonators are shown to hold great promise to achieve high‐performance lasing using colloidal semiconductor nanocrystals (NCs) in solution phase. However, the low packing density of such colloidal gain media in the solution phase results in increased lasing thresholds and poor lasing stability in these WGM lasers. To address these issues, here optical gain in colloidal quantum wells (CQWs) is proposed and shown in the form of high‐density close‐packed solid films constructed around a coreless fiber incorporating the resulting whispering gallery modes to induce gain and waveguiding modes of the fiber to funnel and collect light. In this work, a practical method is presented to produce the first CQW‐WGM laser using an optical fiber as the WGM cavity platform operating at low thresholds of ≈188 µJ cm−2 and ≈1.39 mJ cm−2 under one‐ and two‐photon absorption pumped, respectively, accompanied with a record low waveguide loss coefficient of ≈7 cm−1 and a high net modal gain coefficient of ≈485 cm−1. The spectral characteristics of the proposed CQW‐WGM resonator are supported with a numerical model of full electromagnetic solution. This unique CQW‐WGM cavity architecture offers new opportunities to achieve simple high‐performance optical resonators for colloidal lasers.
Open Access
Emerging fields of colloidal nanophotonics for quality lighting to versatile lasing
(Springer Verlag, 2018) Demir, Hilmi Volkan
Solution-processed semiconductor nanocrystals have attracted increasingly greater interest in optoelectronics including color conversion and enrichment in quality lighting and display backlighting. Optical properties of these colloidal nanocrystals can be conveniently controlled by tailoring their shape, composition, and size in an effort to realize high-performance light generation and lasing. We now witness the expanding deployment of semiconductor nanocrystals in consumer products being adapted by giant electronics companies. Based on the rational design and control of excitonic processes in these nanocrystals, it is possible to achieve highly efficient light-emitting diodes and optically pumped lasers. In this chapter, we introduce an emerging field of nanocrystal optoelectronics with applications from quality lighting to versatile lasing. We look into the performance limits of color conversion using colloidal nanocrystals. Here we introduce a new concept of all-colloidal lasers developed by incorporating nanocrystal emitters as the optical gain media intimately into fully colloidal cavities. As an extreme case of solution-processed tightly-confined quasi-2D colloids, we also show that the atomically flat nanoplatelets uniquely offer record high optical gain coefficients and ultralow threshold stimulated emission. Given the recent accelerating progress in colloidal nanophotonics, solution-processed quantum materials now hold great promise to challenge their conventional epitaxial counterparts in the near future.
Open Access
Excitonics of colloidal nanocrystals for next-generation optoelectronics
(2016-05) Güzeltürk, Burak
Open Access
Future outlook
(Springer, 2019-01) Erdem, Talha; Demir, Hilmi Volkan; Erdem, Talha; Demir, Hilmi Volkan
In this final Chapter, we present a future perspective for the light source design. We discuss the existing problems and briefly introduce new material systems and device architectures that can overcome the current issues.
Open Access
Highly stable, near-unity efficiency atomically flat semiconductor nanocrystals of CdSe/ZnS hetero-nanoplatelets enabled by ZnS-Shell hot-injection growth
(WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, 2019) Yemliha, Yemliha; Quliyeva, Ulviyya; Güngör, Kıvanç; Erdem, Onur; Kelestemur, Yusuf; Mutlugün, Evren; Kovalenko, M.; Demir, Hilmi Volkan
Colloidal semiconductor nanoplatelets (NPLs) offer important benefits in nanocrystal optoelectronics with their unique excitonic properties. For NPLs, colloidal atomic layer deposition (c‐ALD) provides the ability to produce their core/shell heterostructures. However, as c‐ALD takes place at room temperature, this technique allows for only limited stability and low quantum yield. Here, highly stable, near‐unity efficiency CdSe/ZnS NPLs are shown using hot‐injection (HI) shell growth performed at 573 K, enabling routinely reproducible quantum yields up to 98%. These CdSe/ZnS HI‐shell hetero‐NPLs fully recover their initial photoluminescence (PL) intensity in solution after a heating cycle from 300 to 525 K under inert gas atmosphere, and their solid films exhibit 100% recovery of their initial PL intensity after a heating cycle up to 400 K under ambient atmosphere, by far outperforming the control group of c‐ALD shell‐coated CdSe/ZnS NPLs, which can sustain only 20% of their PL. In optical gain measurements, these core/HI‐shell NPLs exhibit ultralow gain thresholds reaching ≈7 µJ cm−2. Despite being annealed at 500 K, these ZnS‐HI‐shell NPLs possess low gain thresholds as small as 25 µJ cm−2. These findings indicate that the proposed 573 K HI‐shell‐grown CdSe/ZnS NPLs hold great promise for extraordinarily high performance in nanocrystal optoelectronics.
Open Access
Introduction
(Springer Singapore, 2022-10-28) Erdem, Onur; Demir, Hilmi Volkan
We begin by giving a short overview of colloidal nanoplatelets, and we explain why their orientation-controlled assemblies are of particular interest. We finalize the chapter by giving an outline of our brief.
Open Access
Ligand exchange and impurity doping in 2d cdse nanoplatelet thin films and their applications
(Wiley-VCH Verlag GmbH & Co. KGaA, 2021-09-23) Lee, W, S.; Kang, Y-G.; Lee, Y. M.; Jean, S.; Sharma, A.; Demir, Hilmi Volkan; Han, M. J.; Koh, W-K.; Oh, S. J.
The effects of halide-ligand exchange and Cu and Ag doping are studied on structural, optical, and electrical properties of four monolayer CdSe nanoplatelet (NPL) and NPL thin films. Combinational study shows that NH4Cl-treatment on CdSe NPL and NPL thin films show tetragonal lattice distortion of NPL, side-to-side attachment between NPLs, bathochromic shift in absorption spectra, and complete quenching of band-edge and dopant-induced emissions. First-principle calculations reveal that Cl creates states below valence band maximum while Ag and Cu dopants create acceptor-like states, explaining the change of their optical property. Field-effect transistors are fabricated to investigate the effect of doping and reduced interplatelet distance on electrical properties of CdSe NPL thin films, demonstrating Cu and Ag dopants mitigate n-type character of CdSe NPL thin films. Temperature-dependent electrical characterization is conducted to further understand charge transport behavior depending on the existence of dopants. This work provides scientific information on the influence of surface chemistry and impurity doping on quantum confined semiconductors and new directions for the design of high-performance nanomaterial-based electronic and optoelectronic devices.
Open Access
Light-Emitting diodes with Cu-Doped colloidal quantum wells: from ultrapure green, tunable dual-emission to white light
(WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, 2019) Liu, B.; Sharma, Manoj; Yu, J.; Shendre, S.; Hettiarachchi, C.; Sharma, Ashma; Yeltik, Aydan; Wang, L.; Sun, H.; Dang, C.; Demir, Hilmi Volkan
Copper‐doped colloidal quantum wells (Cu‐CQWs) are considered a new class of optoelectronic materials. To date, the electroluminescence (EL) property of Cu‐CQWs has not been revealed. Additionally, it is desirable to achieve ultrapure green, tunable dual‐emission and white light to satisfy the various requirement of display and lighting applications. Herein, light‐emitting diodes (LEDs) based on colloidal Cu‐CQWs are demonstrated. For the 0% Cu‐doped concentration, the LED exhibits Commission Internationale de L'Eclairage 1931 coordinates of (0.103, 0.797) with a narrow EL full‐wavelength at half‐maximum of 12 nm. For the 0.5% Cu‐doped concentration, a dual‐emission LED is realized. Remarkably, the dual emission can be tuned by manipulating the device engineering. Furthermore, at a high doping concentration of 2.4%, a white LED based on CQWs is developed. With the management of doping concentrations, the color tuning (green, dual‐emission to white) is shown. The findings not only show that LEDs with CQWs can exhibit polychromatic emission but also unlock a new direction to develop LEDs by exploiting 2D impurity‐doped CQWs that can be further extended to the application of other impurities (e.g., Mn, Ag).
Open Access
Liquid-interface orientation-dictated self-assembly of colloidal semiconductor nanocrystals and its applications
(2023-08) Waris, Mohsin
Over the past, different techniques have been used for the self-assembly of nanocrystals (NCs). Recently, the orientation control over the assembly of anisotropic NCs has been achieved using liquid-interface self-assembly, which is a simple yet vastly applicable technique. Here, we propose and show the first account of the application of this method to assemble multi-layered alternating-orientation NC films, with distinct orientation control of our choice over the NCs in each layer. Being laterally atomically flat, these anisotropic NCs belong to a class of quasi-two-dimensional nanocrystals with one confined dimension. Exhibiting extraordinarily large absorption cross-sections, ultra-narrow emission linewidths, and intrinsic structural anisotropy, these nanoplatelets (NPLs) possess characteristics comparable to those of epitaxially grown quantum wells, though while offering low-cost solution-based synthesis and processability at the same time. Due to this anisotropy, the emission of these NPLs is directional with mostly in-plane transition dipole moments, making them favorable for a variety of optoelectronic active media with orientation control over their deposited films. To achieve this, we have assembled the NPL films with one defined orientation and successfully attained their orientation control using macroscopic parameters, including the evaporation rate of the solvent and subphase selection to be used as the active layers for a number of optoelectronic devices. We demonstrated different multi-layered structures of these NPLs with varying orientations. The resulting surface roughness in all these films was successfully kept, on average, with Sq smoother than 2 nm. We further extended this self-assembly technique to different classes of nanocrystals including large hexagonal NPLs (with around 100 nm in lateral dimensions) and cubic quantum dots (with around 15 nm on each side) to show the versatility of our method. The findings of this thesis indicate that our orientation-dictated self-assembly approach holds great promise for constructing complex colloidal structures made of these oriented nanocrystals as the building blocks.
Embargo
Luminescent solar concentration of type-II nanoplatelets
(2024-08) Özkan, İlayda
The growing demand for renewable energy sources, driven by economic and environmental considerations, has spurred the development of more efficient methods for harnessing solar power. Luminescent solar concentrators (LSCs) are emerging as a promising technology platform owing to their capability to collect and concentrate sunlight delivered to the mounted photovoltaic cells where electrical power is generated. Nanoplatelets (NPLs) draw significant attention as luminophores for LSCs because of our ability to easily alter their optoelectronic properties via tailoring their size, shape, and composition, while making use of advanced architectures of their heterostructures. In this thesis, controlling their composition carefully, CdSe/CdSe1-xTex/CdSe/CdS NPLs in the core/multicrown architecture with type-II band alignment benefitting from their type-II heterostructure’s lower emission energies in the solar spectrum and the suppression of their reabsorption losses were synthesized as the LSC luminophores. The physical characteristics and morphology of these hetero-NPLs were systematically investigated with structural analyses. The resulting CdSe/CdSe1-xTex/CdSe/CdS core/multicrown NPLs having high quantum yields (> 90%), broad Stokes shifts, and stability proved to be excellent candidates for high-performance LSCs. Here, we demonstrated LSC devices fabricated using these type-II NPLs with varied compositions of CdSe/CdSe1-xTex/CdSe/CdS (0.3 ≤ x ≤ 0.6). The best-performing fabricated LSC exhibits an optical power conversion efficiency of 7.29%, the highest reported thus far for NPLs. Thanks to their scalability and affordability, these type-II NPLs hold great promise in several applications of LSCs, including those for agriculture in greenhouses, construction of the facades of buildings, and aerospace together with solar panels on satellites and spacecrafts.
Open Access
Magneto-optical studies of CdSe/CdMnS/CdS core/multi-shell colloidal nanoplatelets
(SPIE, 2016) Petrou, A.; Scrace, T. A.; Murphy, J. R.; Zhang, P.; Norden, T.; Zhang, T.; Thomay, T.; Cartwright, A. N.; Delikanlı, Savaş; Akgül, Mehmet Zafer; Demir, Hilmi Volkan
We studied the photoluminescence (PL)) from CdSe/CdMnS/CdS core/multi-shell colloidal nanoplatelets, a versatile platform to study the interplay of optical properties and nanomagnetism. The photoluminescence (PL) exhibits σ+ polarization in the applied magnetic field. Our measurement detects the presence of even a single magnetic monolayer shell. The PLL consists of a higher and a lower energy component; the latter exhibits a circular polarization peak. The time-resolved PL (trPL) shows a red shift as function of time delay. At early (later) times the trPL spectra coincide with the high (low) energy PL component. A model is proposed to interpret these results.
Open Access
Mn2+-doped CdSe/CdS core/multishell colloidal quantum wells enabling tunable carrier-dopant exchange interactions
(American Chemical Society, 2015) Delikanlı, S.; Akgül, M. Z.; Murphy, J. R.; Barman, B.; Tsai, Y.; Scrace, T.; Zhang, P.; Bozok, B.; Hernández-Martínez, P.L.; Christodoulides, J.; Cartwright, A. N.; Petrou, A.; Demir, Hilmi Volkan
In this work, we report the manifestations of carrier-dopant exchange interactions in colloidal Mn2+-doped CdSe/CdS core/multishell quantum wells. The carrier-magnetic ion exchange interaction effects are tunable through wave function engineering. In our quantum well heterostructures, manganese was incorporated by growing a Cd0.985Mn0.015S monolayer shell on undoped CdSe nanoplatelets using the colloidal atomic layer deposition technique. Unlike previously synthesized Mn2+-doped colloidal nanostructures, the location of the Mn ions was controlled with atomic layer precision in our heterostructures. This is realized by controlling the spatial overlap between the carrier wave functions with the manganese ions by adjusting the location, composition, and number of the CdSe, Cd1-xMnxS, and CdS layers. The photoluminescence quantum yield of our magnetic heterostructures was found to be as high as 20% at room temperature with a narrow photoluminescence bandwidth of ∼22 nm. Our colloidal quantum wells, which exhibit magneto-optical properties analogous to those of epitaxially grown quantum wells, offer new opportunities for solution-processed spin-based semiconductor devices. © 2015 American Chemical Society.
Open Access
Orientation-controlled nonradiative energy transfer to colloidal nanoplatelets: engineering dipole orientation factor
(American Chemical Society, 2019) Erdem, Onur; Güngör, Kıvanç; Güzeltürk, Burak; Tanrıöver, İbrahim; Sak, Mustafa; Olutaş, Murat; Dede, Didem; Kelestemur, Yusuf; Demir, Hilmi Volkan
We proposed and showed strongly orientation-controlled Förster resonance energy transfer (FRET) to highly anisotropic CdSe nanoplatelets (NPLs). For this purpose, we developed a liquid–air interface self-assembly technique specific to depositing a complete monolayer of NPLs only in a single desired orientation, either fully stacked (edge-up) or fully nonstacked (face-down), with near-unity surface coverage and across large areas over 20 cm2. These NPL monolayers were employed as acceptors in an energy transfer working model system to pair with CdZnS/ZnS core/shell quantum dots (QDs) as donors. We found the resulting energy transfer from the QDs to be significantly accelerated (by up to 50%) to the edge-up NPL monolayer compared to the face-down one. We revealed that this acceleration of FRET is accounted for by the enhancement of the dipole–dipole interaction factor between a QD-NPL pair (increased from 1/3 to 5/6) as well as the closer packing of NPLs with stacking. Also systematically studying the distance-dependence of FRET between QDs and NPL monolayers via varying their separation (d) with a dielectric spacer, we found out that the FRET rate scales with d–4 regardless of the specific NPL orientation. Our FRET model, which is based on the original Förster theory, computes the FRET efficiencies in excellent agreement with our experimental results and explains well the enhancement of FRET to NPLs with stacking. These findings indicate that the geometrical orientation of NPLs and thereby their dipole interaction strength can be exploited as an additional degree of freedom to control and tune the energy transfer rate.
Open Access
Record high external quantum efficiency of 19.2% achieved in light-emitting diodes of colloidal quantum wells enabled by hot-Injection shell growth
(WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, 2020) Liu, B.; Altıntaş, Yemliha; Wang, L.; Shendre, S.; Sharma, Manoj; Sun, H.; Mutlugün, Evren; Demir, Hilmi Volkan
Colloidal quantum wells (CQWs) are regarded as a highly promising class of optoelectronic materials, thanks to their unique excitonic characteristics of high extinction coefficients and ultranarrow emission bandwidths. Although the exploration of CQWs in light‐emitting diodes (LEDs) is impressive, the performance of CQW‐LEDs lags far behind other types of soft‐material LEDs (e.g., organic LEDs, colloidal‐quantum‐dot LEDs, and perovskite LEDs). Herein, high‐efficiency CQW‐LEDs reaching close to the theoretical limit are reported. A key factor for this high performance is the exploitation of hot‐injection shell (HIS) growth of CQWs, which enables a near‐unity photoluminescence quantum yield (PLQY), reduces nonradiative channels, ensures smooth films, and enhances the stability. Remarkably, the PLQY remains 95% in solution and 87% in film despite rigorous cleaning. Through systematically understanding their shape‐, composition‐, and device‐engineering, the CQW‐LEDs using CdSe/Cd0.25Zn0.75S core/HIS CQWs exhibit a maximum external quantum efficiency of 19.2%. Additionally, a high luminance of 23 490 cd m−2, extremely saturated red color with the Commission Internationale de L'Eclairage (CIE) coordinates of (0.715, 0.283), and stable emission are obtained. The findings indicate that HIS‐grown CQWs enable high‐performance solution‐processed LEDs, which may pave the path for future CQW‐based display and lighting technologies.